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Interfacing bacteria as biocatalysts with an electrode provides the basis for emerging bioelectrochemical systems that enable sustainable energy interconversion between electrical and chemical energy. Electron transfer rates at the abiotic‐biotic interface are, however, often limited by poor electrical contacts and the intrinsically insulating cell membranes. Herein, we report the first example of an n‐type redox‐active conjugated oligoelectrolyte, namely COE‐NDI, which spontaneously intercalates into cell membranes and mimics the function of endogenous transmembrane electron transport proteins. The incorporation of COE‐NDI into Shewanella oneidensis MR‐1 cells amplifies current uptake from the electrode by 4‐fold, resulting in the enhanced bio‐electroreduction of fumarate to succinate. Moreover, COE‐NDI can serve as a "protein prosthetic" to rescue current uptake in non‐electrogenic knockout mutants. [ABSTRACT FROM AUTHOR]

Bioelectrochemical systems hold the promise of enabling sustainable microbial‐mediated energy interconversion between electrical and chemical energy. Herein, it is demonstrated how a single conjugated polymer can be used to enhance bidirectional extracellular electron transfer through forming self‐assembled coatings on individual cells. Specifically, the n‐type conjugated polyelectrolyte p(cNDI‐gT2) exhibits a reduction potential window between −0.1 and −0.8 V (vs Ag/AgCl), thereby driving thermodynamically favored electron transfer in both directions across the abiotic‐biotic interface that involves the outer membrane cytochromes and flavins of Shewanella oneidensis MR‐1. Electrochemical tests show that injection from an external electrode into Shewanella oneidensis MR‐1 is enabled at negative potentials (−0.6 V), while electron extraction is possible at positive potentials (0.2 V). Relative to controls, the biohybrid shows a sixfold increase in biocurrent generation and a 35‐fold increase in current uptake for the bioelectrosynthesis of succinate from fumarate. This demonstrated abiotic‐biotic synergy provides new strategies for designing multifunctional biohybrids. [ABSTRACT FROM AUTHOR]

Successful practical implementation of bioelectrochemical systems (BES) requires developing affordable electrode structures that promote efficient electrical communication with microbes. Recent efforts have centered on immobilizing bacteria with organic semiconducting polymers on electrodes via electrochemical methods. This approach creates a fixed biocomposite that takes advantage of the increased electrode's electroactive surface area (EASA). Here, it is demonstrated that a biocomposite comprising the water‐soluble conjugated polyelectrolyte CPE‐K and electrogenic Shewanella oneidensis MR‐1 can self‐assemble with carbon paper electrodes, thereby increasing its biocurrent extraction by ≈6‐fold over control biofilms. A ≈1.5‐fold increment in biocurrent extraction is obtained for the biocomposite on carbon paper relative to the biocurrent extracted from gold‐coated counterparts. Electrochemical characterization revealed that the biocomposite stabilized with the carbon paper more quickly than atop flat gold electrodes. Cross‐sectional images show that the biocomposite infiltrates inhomogeneously into the porous carbon structure. Despite an incomplete penetration, the biocomposite can take advantage of the large EASA of the electrode via long‐range electron transport. These results show that previous success on gold electrode platforms can be improved when using more commercially viable and easily manipulated electrode materials. [ABSTRACT FROM AUTHOR]

Power generation and charge storage devices are commonly uncoupled when it comes to the design of materials relevant for their fabrication. Here, it is demonstrated that the biotic–abiotic composite comprising the self‐doped conjugated polyelectrolyte CPE‐K and electrogenic bacteria Shewanella oneidensis MR‐1 can reversibly switch its function between electrical current generation in chronoamperometry mode (≈150 mA m−2) and electrochemical energy storage as a pseudocapacitor with a specific capacitance of up to 80 F g−1. Interconversion of desirable properties for the different functions is achieved by the simple addition and removal of Mg2+ in the bulk electrolyte. Potentiostatic, galvanostatic, and electrochemical impedance spectroscopy characterization, accompanied by imaging and cell viability tests, indicate that the modulation of properties is a result of reversible changes in CPE‐K macrostructures and in the number of living bacteria within the composite. The results show the possibility to realize an "on‐demand" switch between current generation and charge storage by one integrated "living" material. [ABSTRACT FROM AUTHOR]

The high electrical conductivity and low dimensionality of graphene is essential for the development of novel lightweight bioanodes for new-generation energy technologies. However, the integration of graphene in biointerfaces presents a formidable challenge, especially because the surface energy of graphene is not compatible with living matter. Here we propose a sustainable chemical control method to reach the demanded surface hydrophilicity and conductivity of graphene nanowalls to form a lightweight, graphene-based, sponge bioanode. The few-nanometer–thick conductive graphene nanowalls create biocompatible hydrophilic microconfinements to harvest the biomass density of electrogenic Shewanella Oneidensis MR-1. The graphene-based bioanode shows a stable and rapid response with a steady-state biocurrent density of 135.35 mA m−2 realized within a few hours. Our novel and sustainable graphene-based material provides a revolutionary energy opportunity for the establishment of new energy-related graphene industries as well as facilitates many startups. A facile and chemical-free method was leveraged to produce the graphene-based bioanode. Balancing the hydrophilicity and conductivity of the graphene nanowalls was achieved by simply tuning its reduction temperature and was the first time, revealed to play an important role in the performance of the microbial electrode. A steady-state bio-current density of 135.35 mA m−2 was realized within a few hours and with long-term duration. [Display omitted] [ABSTRACT FROM AUTHOR]